Sequential *CO management via controlling in situ reconstruction for efficient industrial-current-density CO2-to-C2+ electroreduction.

Sequentially managing the coverage and dimerization of *CO on the Cu catalysts is desirable for industrial-current-density CO2 reduction (CO2R) to C2+, which required the multiscale design of the surface atom/architecture. However, the oriented design is colossally difficult and even no longer valid due to unpredictable reconstruction. Here, we leverage the synchronous leaching of ligand molecules to manipulate the seeding-growth process during CO2R reconstruction and construct Cu arrays with favorable (100) facets. The gradient diffusion in the reconstructed array guarantees a higher *CO coverage, which can continuously supply the reactant to match its high-rate consumption for high partial current density for C2+. Sequentially, the lower energy barriers of *CO dimerization on the (100) facets contribute to the high selectivity of C2+. Profiting from this sequential *CO management, the reconstructed Cu array delivers an industrial-relevant FEC2+ of 86.1% and an FEC2H4 of 60.8% at 700 mA cm-2. Profoundly, the atomic-molecular scale delineation for the evolution of catalysts and reaction intermediates during CO2R can undoubtedly facilitate various electrocatalytic reactions.

Langmuir-Blodgett Film Formed by Amphiphilic Molecules for Facile and Rapid Construction of Zinc-Iodine Cell.

Zinc-iodine batteries (ZIBs) are promising candidates for ecofriendly, safe, and low-cost energy storage systems, but polyiodide shuttling and the complex cathode fabrication procedures have severely hindered their broader commercial usage. Herein, a protocol is developed using phospholipid-like oleylamine molecules for scalable production of Langmuir-Blodgett films, which allows the facile preparation of ZIB cathodes in less than 1 min. The resulting inhomogeneous cathode allows for the continuous conversion of iodine. Moreover, the amine group of the oleylamine molecule at the cathode is capable of producing [OA*I+]I3- charge-transfer complexes with iodine, which facilitates the rapid migration of iodine and results in a highly reversible iodine conversion process. Consequently, the as-prepared ZIBs can deliver over 2000 cycles at 0.5 mA cm-2 with a capacity retention of 75.3%. This work presents a novel, straightforward, and efficient method for the rapid construction of ZIBs.

Interfacial Accumulation and Stability Enhancement Effects Triggered by Built-in Electric Field of SnO2/LaOCl Nanofibers Boost Carbon Dioxide Electroreduction.

Constructing a built-in interfacial electric field (BIEF) is an effective approach to enhance the electrocatalysts performance, but it has been rarely demonstrated for electrochemical carbon dioxide reduction reaction (CO2RR) to date. Herein, for the first time, SnO2/LaOCl nanofibers (NFs) with BIEF is created by electrospinning, exhibiting a high Faradaic efficiency (FE) of 100% C1 product (CO and HCOOH) at -0.9--1.1 V versus reversible hydrogen electrode (RHE) and a maximum FEHCOOH of 90.1% at -1.2 VRHE in H-cell, superior to the commercial SnO2 nanoparticles (NPs) and LaOCl NFs. SnO2/LaOCl NFs also exhibit outstanding stability, maintaining negligible activity degradation even after 10 h of electrolysis. Moreover, their current density and FEHCOOH are almost 400 mA cm-2 at -2.31 V and 83.4% in flow-cell. The satisfactory CO2RR performance of SnO2/LaOCl NFs with BIEF can be ascribed to tight interface of coupling SnO2 NPs and LaOCl NFs, which can induce charge redistribution, rich active sites, enhanced CO2 adsorption, as well as optimized Gibbs free energy of *OCHO. The work reveals that the BIEF will trigger interfacial accumulation and stability enhancement effects in promoting CO2RR activity and stability of SnO2-based materials, providing a novel approach to develop stable and efficient CO2RR electrocatalysts.

Inducing Directional Charge Delocalization in 3D-Printable Micro-Supercapacitors Based on Strongly Coupled Black Phosphorus and ReS2 Nanocomposites.

The growing interest in so-called interface coupling strategies arises from their potential to enhance the performance of active electrode materials. Nevertheless, designing a robust coupled interface in nanocomposites for stable electrochemical processes remains a challenge. In this study, an epitaxial growth strategy is proposed by synthesizing sulfide rhenium (ReS2 ) on exfoliated black phosphorus (E-BP) nanosheets, creating an abundance of robust interfacial linkages. Through spectroscopic analysis using X-ray photoelectron spectroscopy and X-ray absorption spectroscopy, the authors investigate the interfacial environment. The well-developed coupled interface and structural stability contribute to the impressive performance of the 3D-printed E-BP@ReS2 -based micro-supercapacitor, achieving a specific capacitance of 47.3 mF cm-2 at 0.1 mA cm-2 and demonstrating excellent long-term cyclability (89.2% over 2000 cycles). Furthermore, density functional theory calculations unveil the positive impact of the strongly coupled interface in the E-BP@ReS2 nanocomposite on the adsorption of H+ ions, showcasing a significantly reduced adsorption energy of -2.17 eV. The strong coupling effect facilitates directional charge delocalization at the interface, enhancing the electrochemical performance of electrodes and resulting in the successful construction of advanced micro-supercapacitors.

Anti-Freezing Electrolytes in Aqueous Multivalent Metal-Ion Batteries: Progress, Challenges, and Optimization Strategies.

Aqueous rechargeable multivalent metal-ion batteries (ARMMBs) have attracted considerable attention due to their high capacity, high energy density, and low cost. However, their performance is often limited by low temperature operation, which requires the development of anti-freezing electrolytes. In this review, we summarize the anti-freezing mechanisms and optimization strategies of anti-freezing electrolytes for aqueous batteries (especially for Zn-ion batteries). Besides, we investigate the possible interactions and side reactions between electrolytes and electrodes. We also analyze the problems between electrolytes and electrodes at low temperature, and propose possible solutions. The research progress in the field of low temperature energy storage for aqueous Mg-ion, Ca-ion, and Al-ion batteries, and the challenges faced in their anti-freezing electrolytes are investigated in detail. Last but not least, the outlook on the energy storage applications of ARMMBs is provided to guide the future research.

Human Skin-Mimicking Ionogel-Based Electronic Skin for Intelligent Robotic Sorting.

Creating bionic intelligent robotic systems that emulate human-like skin perception presents a considerable scientific challenge. This study introduces a multifunctional bionic electronic skin (e-skin) made from polyacrylic acid ionogel (PAIG), designed to detect human motion signals and transmit them to robotic systems for recognition and classification. The PAIG was synthesized using a suspension of liquid metal and graphene oxide nanosheets as initiators and cross-linkers. The resulting PAIGs demonstrate excellent mechanical properties, resistance to freezing and drying, and self-healing capabilities. Functionally, the PAIG effectively captures human motion signals through electromechanical sensing. Furthermore, we developed a bionic intelligent sorting robot system by integrating the PAIG-based e-skin with a robotic manipulator. This system leverages its ability to detect frictional electrical signals, enabling precise identification and sorting of materials. The innovations presented in this study hold significant potential for applications in artificial intelligence, rehabilitation training, and intelligent classification systems. This article is protected by copyright. All rights reserved.

Cation Substitution Strategy for Developing Perovskite Oxide with Rich Oxygen Vacancy-Mediated Charge Redistribution Enables Highly Efficient Nitrate Electroreduction to Ammonia.

The electrocatalytic nitrate (NO3-) reduction reaction (eNITRR) is a promising method for ammonia synthesis. However, its efficacy is currently limited due to poor selectivity, largely caused by the inherent complexity of the multiple-electron processes involved. To address these issues, oxygen-vacancy-rich LaFe0.9M0.1O3-δ (M = Co, Ni, and Cu) perovskite submicrofibers have been designed from the starting material LaFeO3-δ (LF) by a B-site substitution strategy and used as the eNITRR electrocatalyst. Consequently, the LaFe0.9Cu0.1O3-δ (LF0.9Cu0.1) submicrofibers with a stronger Fe-O hybridization, more oxygen vacancies, and more positive surface potential exhibit a higher ammonia yield rate of 349 ± 15 µg h-1 mg-1cat. and a Faradaic efficiency of 48 ± 2% than LF submicrofibers. The COMSOL Multiphysics simulations demonstrate that the more positive surface of LF0.9Cu0.1 submicrofibers can induce NO3- enrichment and suppress the competing hydrogen evolution reaction. By combining a variety of in situ characterizations and density functional theory calculations, the eNITRR mechanism is revealed, where the first proton-electron coupling step (*NO3 + H+ + e- → *HNO3) is the rate-determining step with a reduced energy barrier of 1.83 eV. This work highlights the positive effect of cation substitution in promoting eNITRR properties of perovskites and provides new insights into the studies of perovskite-type electrocatalytic ammonia synthesis catalysts.

Perovskites with Enriched Oxygen Vacancies as a Family of Electrocatalysts for Efficient Nitrate Reduction to Ammonia.

Electrochemical nitrate reduction to ammonia (NRA) provides an efficient, sustainable approach to convert the nitrate pollutants into value-added products, which is regarded as a promising alternative to the industrial Haber-Bosch process. Recent studies have shown that oxygen vacancies of oxide catalysts can adjust the adsorption energies of intermediates and affect their catalytic performance. Compared with other metal oxides, perovskite oxides can allow their metal cations to exist in abnormal or mixed valence states, thereby resulting in enriched oxygen vacancies in their crystal structures. Here, the catalytic activities of perovskite oxides toward NRA catalysis with respect to the amount of oxygen vacancies are explored, where four perovskite oxides with different crystal structures (including cubic LaCrO3 , orthorhombic LaMnO3 and LaFeO3 , hexagonal LaCoO3 ) are chosen and investigated. By combining X-ray photoelectron spectroscopy, electron paramagnetic resonance spectroscopy and electrochemical measurements, it is found that the amount of oxygen vacancies in these perovskite oxides surprisingly follow the same order as their activities toward NRA catalysis (LaCrO3  < LaMnO3  < LaFeO3  < LaCoO3 ). Further theoretical studies reveal that the existence of oxygen vacancies in LaCoO3 perovskite can decrease the energy barriers for reduction of *HNO3 to *NO2 , leading to its superior NRA performance.

Quasi-Homogeneous and Hierarchical Electronic Textiles with Porosity-Hydrophilicity Dual-Gradient for Unidirectional Sweat Transport, Electrophysiological Monitoring, and Body-Temperature Visualization.

On-skin electronics based on impermeable elastomers and stacking structures often suffer from inferior sweat-repelling capabilities and severe mechanical mismatch between sub-layers employed, which significantly impedes their lengthy wearing comfort and functionality. Herein, inspired by the transpiration system of vascular plants and the water diode phenomenon, a hierarchical nonwoven electronic textile (E-textile) with multi-branching microfibers and robust interlayer adhesion is rationally developed. The layer-by-layer electro-airflow spinning method and selective oxygen plasma treatment are utilized to yield a porosity-hydrophilicity dual-gradient. The resulting E-textile shows unidirectional, nonreversible, and anti-gravity water transporting performance even upon large-scale stretching (250%), excellent mechanical matching between sub-layers, as well as a reversible color-switching ability to visualize body temperature. More importantly, the conducting and skin-conformal E-textile demonstrates accurate and stable detecting capability for biomechanical and bioelectrical signals when applied as an on-skin bioelectrode, including different human activities, electrocardiography, electromyogram, and electrodermal activity signals. Further, the E-textile can be efficiently implemented in human-machine interfaces to build a gesture-controlled dustbin and a smart acousto-optic alarm. Hence, this hierarchically-designed E-textile with integrated functionalities offers a practical and innovative method for designing comfortable and daily applicable on-skin electronics.

Xylem-Inspired Polyimide/MXene Aerogels with Radial Lamellar Architectures for Highly Sensitive Strain Detection and Efficient Solar Steam Generation.

Polyimide aerogels with mechanical robustness, great compressibility, excellent antifatigue properties, and intriguing functionality have captured enormous attention in diverse applications. Here, enlightened by the xylem parenchyma of dicotyledonous stems, a radially architectured polyimide/MXene composite aerogel (RPIMX) with reversible compressibility is developed by combining the interfacial enhancing strategy and radial ice-templating method. The strong interaction between MXene flakes and polymer can glue the MXene to form continuous lamellae, the ice crystals grow preferentially along the radial temperature gradient can effectively constrain the lamellae to create a biomimetic radial lamellar architecture. As a result, the nature-inspired RPIMX composite aerogel with centrosymmetric lamellar structure and oriented channels manifests excellent mechanical strength, electrical conductivity, and water transporting capability along the longitudinal direction, endowing itself with intriguing applications for accurate human motion monitoring and efficient photothermal evaporation. These exciting properties make the biomimetic RPIMX aerogels promising candidates for flexible piezoresistive sensors and photothermal evaporators.

Bio-Inspired Aerobic-Hydrophobic Janus Interface on Partially Carbonized Iron Heterostructure Promotes Bifunctional Nitrogen Fixation.

Competition from hydrogen/oxygen evolution reactions and low solubility of N2 in aqueous systems limited the selectivity and activity on nitrogen fixation reaction. Herein, we design an aerobic-hydrophobic Janus structure by introducing fluorinated modification on porous carbon nanofibers embedded with partially carbonized iron heterojunctions (Fe3 C/Fe@PCNF-F). The simulations prove that the Janus structure can keep the internal Fe3 C/Fe@PCNF-F away from water infiltration and endow a N2 molecular-concentrating effect, suppressing the competing reactions and overcoming the mass-transfer limitations to build a robust "quasi-solid-gas" state micro-domain around the catalyst surface. In this proof-of-concept system, the Fe3 C/Fe@PCNF-F exhibits excellent electrocatalytic performance for nitrogen fixation (NH3 yield rate up to 29.2 µg h-1 mg-1 cat. and Faraday efficiency (FE) up to 27.8 % in nitrogen reduction reaction; NO3 - yield rate up to 15.7 µg h-1 mg-1 cat. and FE up to 3.4 % in nitrogen oxidation reaction).

Lattice Strained B-Doped Ni Nanoparticles for Efficient Electrochemical H2 O2 Synthesis.

Surface strains are necessary to optimize the oxygen adsorption energy during the oxygen reduction reaction (ORR) in the four-electron process, but the surface strains regulation for ORR in the two-electron process to produce hydrogen peroxide (H2 O2 ) is rarely studied. Herein, it is reported that the tensile strained B-doped Ni nanoparticles on carbon support (Ni-B@BNC) could enhance the adsorption of O2 , stabilize OO bond, and boost the electrocatalytic ORR to H2 O2 . Moreover, the Ni-B@BNC catalysts exhibit volcano-type activity for electrocatalytic ORR to H2 O2 as a function of the strain intensity, which is controlled by B content. Among them, Ni4 -B1 @BNC exhibits the highest H2 O2 selectivity of over 86%, H2 O2 yield of 128.5 mmol h-1  g-1 , and Faraday efficiency of 94.9% at 0.6 V vs reversible hydrogen electrode as well as durable stability after successive cycling, being one of the state-of-the-art electrocatalysts for two-electron ORR. The density functional theory calculations reveal that tensile strain introduced by doping B into Ni nanoparticles could decrease the state density of Ni-3d orbital and optimize the binding energy of OOH* during ORR. A new direction is provided here for the design of highly active and stable catalysts for potential H2 O2 production and beyond.

Site-Sensitive Selective CO2 Photoreduction to CO over Gold Nanoparticles.

We demonstrate a new case of materials-gene engineering to precisely design photocatalysts with the prescribed properties. Based on theoretical calculations, a phase-doping strategy was proposed to regulate the pathways of CO2 conversion over Au nanoparticles (NPs) loaded TiO2 photocatalysts. As a result, the thermodynamic bottleneck of CO2 -to-CO conversion is successfully unlocked by the incorporation of stable twinning crystal planes into face-centered cubic (fcc) phase Au NPs. Compared to bare pristine TiO2 , the activity results showed that the loading of regular fcc-Au NPs raised the CO production by 18-fold but suppressed the selectivity from 84 % to 75 %, whereas Au NPs with twinning (110) and (100) facets boosted the activity by nearly 40-fold and established near unity CO selectivity. This enhancement is shown to originate from a beneficial shift in the surface reactive site energetics arising at the twinned stacking fault, whereby both the CO reaction energy and desorption energy were significantly reduced.

Constructing Interfacial Boron-Nitrogen Moieties in Turbostratic Carbon for Electrochemical Hydrogen Peroxide Production.

The electrochemical oxygen reduction reaction (ORR) provides a green route for decentralized H2 O2 synthesis, where a structure-selectivity relationship is pivotal for the control of a highly selective and active two-electron pathway. Here, we report the fabrication of a boron and nitrogen co-doped turbostratic carbon catalyst with tunable B-N-C configurations (CNB-ZIL) by the assistance of a zwitterionic liquid (ZIL) for electrochemical hydrogen peroxide production. Combined spectroscopic analysis reveals a fine tailored B-N moiety in CNB-ZIL, where interfacial B-N species in a homogeneous distribution tend to segregate into hexagonal boron nitride domains at higher pyrolysis temperatures. Based on the experimental observations, a correlation between the interfacial B-N moieties and HO2 - selectivity is established. The CNB-ZIL electrocatalysts with optimal interfacial B-N moieties exhibit a high HO2 - selectivity with small overpotentials in alkaline media, giving a HO2 - yield of ≈1787 mmol gcatalyst -1 h-1 at -1.4 V in a flow-cell reactor.

N2 Electroreduction to NH3 by Selenium Vacancy-Rich ReSe2 Catalysis at an Abrupt Interface.

Vacancy engineering has been proved repeatedly as an adoptable strategy to boost electrocatalysis, while its poor selectivity restricts the usage in nitrogen reduction reaction (NRR) as overwhelming competition from hydrogen evolution reaction (HER). Revealed by density functional theory calculations, the selenium vacancy in ReSe2 crystal can enhance its electroactivity for both NRR and HER by shifting the d-band from -4.42 to -4.19 eV. To restrict the HER, we report a novel method by burying selenium vacancy-rich ReSe2 @carbonized bacterial cellulose (Vr -ReSe2 @CBC) nanofibers between two CBC layers, leading to boosted Faradaic efficiency of 42.5 % and ammonia yield of 28.3 µg h-1 cm-2 at a potential of -0.25 V on an abrupt interface. As demonstrated by the nitrogen bubble adhesive force, superhydrophilic measurements, and COMSOL Multiphysics simulations, the hydrophobic and porous CBC layers can keep the internal Vr -ReSe2 @CBC nanofibers away from water coverage, leaving more unoccupied active sites for the N2 reduction (especially for the potential determining step of proton-electron coupling and transferring processes as *NN → *NNH).

Multidimensional Integrated Chalcogenides Nanoarchitecture Achieves Highly Stable and Ultrafast Potassium-Ion Storage.

Potassium-ion batteries (KIBs) have come into the spotlight in large-scale energy storage systems because of cost-effective and abundant potassium resources. However, the poor rate performance and problematic cycle life of existing electrode materials are the main bottlenecks to future potential applications. Here, the first example of preparing 3D hierarchical nanoboxes multidimensionally assembled from interlayer-expanded nano-2D MoS2 @dot-like Co9 S8 embedded into a nitrogen and sulfur codoped porous carbon matrix (Co9 S8 /NSC@MoS2 @NSC) for greatly boosting the electrochemical properties of KIBs in terms of reversible capacity, rate capability, and cycling lifespan, is reported. Benefiting from the synergistic effects, Co9 S8 /NSC@MoS2 @NSC manifest a very high reversible capacity of 403 mAh g-1 at 100 mA g-1 after 100 cycles, an unprecedented rate capability of 141 mAh g-1 at 3000 mA g-1 over 800 cycles, and a negligible capacity decay of 0.02% cycle-1 , boosting promising applications in high-performance KIBs. Density functional theory calculations demonstrate that Co9 S8 /NSC@MoS2 @NSC nanoboxes have large adsorption energy and low diffusion barriers during K-ion storage reactions, implying fast K-ion diffusion capability. This work may enlighten the design and construction of advanced electrode materials combined with strong chemical bonding and integrated functional advantages for future large-scale stationary energy storage.

Tailoring the Grain Boundary Chemistry of Polymeric Carbon Nitride for Enhanced Solar Hydrogen Production and CO2 Reduction.

Photocatalytic water splitting is a promising and clean way to mimic plant photosynthesis in a sustainable manner. Improvements of the quantum efficiency and optical absorption in the relevant range are necessary steps to approach practicality. Herein, we reported that these issues can be readily addressed when 5-aminotetrazole, a monomer with high nitrogen content, is used for the synthesis of carbon nitride. The molten salt mixture NaCl/KCl is used as a high-temperature solvent to tailor the grain boundary structure and chemistry. Visible light quantum efficiency for H2 production of 0.65 could be obtained in the presence of K2 HPO4 as a double layer modifier. This value is very high, considering that this number depends on light to charge couple conversion, charge localization, as well as a successful oxidation and reduction reaction.

Sulfur-Deficient Bismuth Sulfide/Nitrogen-Doped Carbon Nanofibers as Advanced Free-Standing Electrode for Asymmetric Supercapacitors.

The use of free-standing carbon-based hybrids plays a crucial role to help fulfil ever-increasing energy storage demands, but is greatly hindered by the limited number of active sites for fast charge adsorption/desorption processes. Herein, an efficient strategy is demonstrated for making defect-rich bismuth sulfides in combination with surface nitrogen-doped carbon nanofibers (dr-Bi2 S3 /S-NCNF) as flexible free-standing electrodes for asymmetric supercapacitors. The dr-Bi2 S3 /S-NCNF composite exhibits superior electrochemical performances with an enhanced specific capacitance of 466 F g-1 at a discharge current density of 1 A g-1 . The high performance of dr-Bi2 S3 /S-NCNF electrodes originates from its hierarchical structure of nitrogen-doped carbon nanofibers with well-anchored defect-rich bismuth sulfides nanostructures. As modeled by density functional theory calculation, the dr-Bi2 S3 /S-NCNF electrodes exhibit a reduced OH- adsorption energy of -3.15 eV, compared with that (-3.06 eV) of defect-free bismuth sulfides/surface nitrogen-doped carbon nanofiber (df-Bi2 S3 /S-NCNF). An asymmetric supercapacitor is further fabricated by utilizing dr-Bi2 S3 /S-NCNF hybrid as the negative electrode and S-NCNF as the positive electrode. This composite exhibits a high energy density of 22.2 Wh kg-1 at a power density of 677.3 W kg-1 . This work demonstrates a feasible strategy to construct advanced metal sulfide-based free-standing electrodes by incorporating defect-rich structures using surface engineering principles.

Bionanofiber Assisted Decoration of Few-Layered MoSe2 Nanosheets on 3D Conductive Networks for Efficient Hydrogen Evolution.

Molybdenum diselenide (MoSe2 ) has emerged as a promising electrocatalyst for hydrogen evolution reaction (HER). However, its properties are still confined due to the limited active sites and poor conductivity. Thus, it remains a great challenge to synergistically achieve structural and electronic modulations for MoSe2 -based HER catalysts because of the contradictory relationship between these two characteristics. Herein, bacterial cellulose-derived carbon nanofibers are used to assist the uniform growth of few-layered MoSe2 nanosheets, which effectively increase the active sites of MoSe2 for hydrogen atom adsorption. Meanwhile, carbonized bacterial cellulose (CBC) nanofibers provide a 3D network for electrolyte penetration into the inner space and accelerate electron transfer as well, thus leading to the dramatically increased HER activity. In acidic media, the CBC/MoSe2 hybrid catalyst exhibits fast hydrogen evolution kinetics with onset overpotential of 91 mV and Tafel slope of 55 mV dec-1 , which is much more outstanding than both bulk MoSe2 aggregates and CBC nanofibers. Furthermore, the fast HER kinetics are well supported by theoretical calculations of density-functional-theory analysis with a low activation barrier of 0.08 eV for H2 generation. Hence, this work highlights an efficient solution to develop high-performance HER catalysts by incorporating biotemplate materials, to simultaneously achieve increased active sites and conductivity.

Biomass-Derived Nitrogen-Doped Carbon Nanofiber Network: A Facile Template for Decoration of Ultrathin Nickel-Cobalt Layered Double Hydroxide Nanosheets as High-Performance Asymmetric Supercapacitor Electrode.

The development of biomass-based energy storage devices is an emerging trend to reduce the ever-increasing consumption of non-renewable resources. Here, nitrogen-doped carbonized bacterial cellulose (CBC-N) nanofibers are obtained by one-step carbonization of polyaniline coated bacterial cellulose (BC) nanofibers, which not only display excellent capacitive performance as the supercapacitor electrode, but also act as 3D bio-template for further deposition of ultrathin nickel-cobalt layered double hydroxide (Ni-Co LDH) nanosheets. The as-obtained CBC-N@LDH composite electrodes exhibit significantly enhanced specific capacitance (1949.5 F g(-1) at a discharge current density of 1 A g(-1) , based on active materials), high capacitance retention of 54.7% even at a high discharge current density of 10 A g(-1) and excellent cycling stability of 74.4% retention after 5000 cycles. Furthermore, asymmetric supercapacitors (ASCs) are constructed using CBC-N@LDH composites as positive electrode materials and CBC-N nanofibers as negative electrode materials. By virtue of the intrinsic pseudocapacitive characteristics of CBC-N@LDH composites and 3D nitrogen-doped carbon nanofiber networks, the developed ASC exhibits high energy density of 36.3 Wh kg(-1) at the power density of 800.2 W kg(-1) . Therefore, this work presents a novel protocol for the large-scale production of biomass-derived high-performance electrode materials in practical supercapacitor applications.